EP1136671B1 - Verfahren zur Überprüfung der Funktionstüchtigkeit eines Abgasreinigungskatalysators - Google Patents
Verfahren zur Überprüfung der Funktionstüchtigkeit eines Abgasreinigungskatalysators Download PDFInfo
- Publication number
- EP1136671B1 EP1136671B1 EP01106782A EP01106782A EP1136671B1 EP 1136671 B1 EP1136671 B1 EP 1136671B1 EP 01106782 A EP01106782 A EP 01106782A EP 01106782 A EP01106782 A EP 01106782A EP 1136671 B1 EP1136671 B1 EP 1136671B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- catalyst
- carbon monoxide
- engine
- exhaust gas
- temperature
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
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Classifications
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N11/00—Monitoring or diagnostic devices for exhaust-gas treatment apparatus, e.g. for catalytic activity
- F01N11/002—Monitoring or diagnostic devices for exhaust-gas treatment apparatus, e.g. for catalytic activity the diagnostic devices measuring or estimating temperature or pressure in, or downstream of the exhaust apparatus
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N11/00—Monitoring or diagnostic devices for exhaust-gas treatment apparatus, e.g. for catalytic activity
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N11/00—Monitoring or diagnostic devices for exhaust-gas treatment apparatus, e.g. for catalytic activity
- F01N11/002—Monitoring or diagnostic devices for exhaust-gas treatment apparatus, e.g. for catalytic activity the diagnostic devices measuring or estimating temperature or pressure in, or downstream of the exhaust apparatus
- F01N11/005—Monitoring or diagnostic devices for exhaust-gas treatment apparatus, e.g. for catalytic activity the diagnostic devices measuring or estimating temperature or pressure in, or downstream of the exhaust apparatus the temperature or pressure being estimated, e.g. by means of a theoretical model
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N2550/00—Monitoring or diagnosing the deterioration of exhaust systems
- F01N2550/02—Catalytic activity of catalytic converters
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
- F02B—INTERNAL-COMBUSTION PISTON ENGINES; COMBUSTION ENGINES IN GENERAL
- F02B3/00—Engines characterised by air compression and subsequent fuel addition
- F02B3/06—Engines characterised by air compression and subsequent fuel addition with compression ignition
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
- Y02T10/10—Internal combustion engine [ICE] based vehicles
- Y02T10/40—Engine management systems
Definitions
- the invention relates to a method for checking the functionality of a catalyst for the purification of the exhaust gases of an internal combustion engine.
- the process is particularly suitable for monitoring a diesel oxidation catalyst.
- the functionality of the catalyst is monitored according to the invention by measuring the conversion of carbon monoxide in combination with a temperature measurement.
- the process is also suitable for monitoring the performance of HC-DeNO x and urea-SCR catalysts and NO x adsorber catalysts.
- OBD system on-board diagnostic system
- Malfunctions of one or more Components of the exhaust system are signaled by the illumination of a warning lamp.
- OBD system On-board diagnostic system
- Object of the present invention is therefore to provide a method for checking the Specify functional efficiency of an exhaust gas purification catalyst, which also for the verification of the function of oxidation catalysts suitable for diesel engines is and the determination of the catalyst activity directly via the measurement of the implementation allowed by carbon monoxide (CO).
- CO carbon monoxide
- the light-off temperature for the carbon monoxide oxidation is understood to mean the temperature T CO, 50% , at which carbon monoxide is just about 50% reacted.
- the catalytic activity of the catalyst still remaining after a certain period of operation is assessed directly.
- the characteristic variables for this are the degree of conversion r CO for carbon monoxide, the current exhaust gas exit temperature T A and the fresh preheat temperature for CO, T CO, 50%, fresh , which is a function of the speed and the load and stored in advance in the OBD electronics can be.
- c CO
- 2 the measured concentration of carbon monoxide in the exhaust gas downstream of the catalyst
- c CO
- 1 the measured concentration of carbon monoxide in the exhaust gas upstream of the catalyst.
- r CO 1 - c CO, 2 c CO, engine .
- c CO, 2 is the measured concentration of carbon monoxide in the exhaust gas downstream of the catalyst and c CO, engine is the carbon monoxide concentration stored in the OBD electronics as a map for the current engine operating point.
- the pollutant conversion of a catalyst is, to a maximum, of its Temperature dependent. It shows a catalyst for each of the three gaseous Main pollutants CO, HC (hydrocarbons) and NOx (nitrogen oxides) another Temperature profile of the pollutant conversion.
- CO gaseous Main pollutants
- HC hydrocarbons
- NOx nitrogen oxides
- the reaction For carbon monoxide and the hydrocarbons, the reaction increases in a narrow temperature range by the relevant light-off temperature T CO, 50%, or T HC, 50% strong and then approaches the maximum degree of conversion.
- T CO light-off temperature
- T HC light-off temperature
- the reaction for nitrogen oxides at low temperatures is close to zero. It reaches a maximum in the range of light-off temperature for hydrocarbons T HC, 50%, and drops again to near zero at high catalyst temperatures.
- CO oxidation has proven particularly critical for aging effects in diesel oxidation catalysts (FIG. 2).
- the assessment of catalysts for CO oxidation capability is therefore well suited for diesel applications because current (diesel oxidation catalyst) and future diesel exhaust aftertreatment systems (HC-DeNOx, NOx adsorber, urea-SCR) rely largely on platinum as the catalytically active material.
- the activity of the platinum catalysts in all cases depends very much on the platinum particle size.
- the deterioration in the activity of the catalysts after aging is due to an increase in the catalytically active platinum particles and the concomitant loss of catalytically active surface.
- CO oxidation is the reaction that detects these changes very precisely.
- HC has the advantage of being a well-defined chemical compound which is identical for all engine operating points.
- HC is a Mixture of substances, the composition of which depends on the engine operating point. An exact metrological detection is thus more complicated compared to CO.
- CO as indicator pollutant compared to HC is the difference Definition of emission limit values according to European emission legislation founded. While there are separate limits for CO, NOx and particulate matter the limits for HC are defined only for the sum of HC and NOx. Therefore, the hang tolerable HC emissions from the current NOx emissions. The choice of HC as the sole indicator pollutant is therefore unfavorable.
- the carbon monoxide concentration c CO, 2 in the exhaust gas behind the catalyst is determined according to the invention by a built-in behind the converter in the exhaust gas line carbon monoxide sensor.
- the carbon monoxide concentration c CO, 1 before the catalyst can also be measured directly with a carbon monoxide sensor or taken from the previously stored in the OBD electronics for each engine operating point as a map values.
- the raw emissions of the engine type used are determined in advance for all engine operating points and stored as concentration values as a function of speed and load in the OBD electronics.
- concentration values taken from the memory of the OBD electronics, which correspond to the engine's raw emission values, are referred to below as c CO, engine .
- the degree of conversion of the pollutant is calculated in this case according to equation (3).
- the engine operating data that is the in the measurement and Calculation present operating point, continuously from the engine electronics to the OBD electronics transmitted.
- the current exhaust gas temperature T A is measured downstream of the catalyst by a temperature sensor and determines the degree of conversion r CO for carbon monoxide for the corresponding temperature to assess the state of the catalyst.
- the determination of r CO according to equation (3) from C CO, 2 and the data c CO, motor stored as a map here has the advantage over the favorable cost that the quotient of two sensor signals of very different magnitude are not formed compared to the measurement of both concentration values got to.
- the sensor in front of the catalyst is constantly exposed to a different gas atmosphere as the sensor behind the catalyst, which would lead to a different aging of the sensors, which would have to be considered in the calculation of the degree of conversion.
- the temperature measurement takes place behind the catalytic converter, in dynamic driving mode to ensure that the measured exhaust gas temperature is the actual catalyst temperature equivalent. This would be in the measurement of the exhaust gas temperature before the catalyst due to its thermal inertia during cold start and fast load changes not guaranteed.
- the light-off temperature T CO, 50%, fresh is a function of all pollutant concentrations, that is, the raw emissions of the engine, and the space velocity in the catalytic converter.
- the raw emissions of the engine and the space velocity within the converter are functions of load and speed.
- the light-off temperatures T CO, 50%, fresh for all engine operating points are therefore stored as a function of load and speed in the OBD electronics as a map.
- the Grenzum aptitudesgrad r CO, G may for example be 50%.
- the catalytic converter is therefore only judged to be permanently damaged if a malfunction is detected for several operating points of the engine.
- the engine control maps are generally permanently stored with the operating data of the engine for a grid of discrete operating points. Not all of these operating points are equally well suited to assessing the functionality of the catalyst. Thus, for example, operating points with high exhaust gas temperatures are unsuitable, since even a damaged catalyst can still deliver good conversions for carbon monoxide at high exhaust gas temperatures. For the assessment of the catalyst, therefore, preference is given to using only a selection from the possible operating points, which are particularly critical.
- the number of operating points selected for the evaluation of the catalyst is referred to below as n a .
- the catalyst is considered severely damaged if a malfunction is detected for a certain number n F of the selected operating points.
- the operating points for which a malfunction is determined and their number can be stored and accumulated over several driving cycles. Only when the number n F of operating points with malfunctions is exceeded, a signal for replacing the catalyst is set.
- a further safeguard against a premature classification of the catalyst as damaged can be obtained if it is determined that the number n F of operating points with malfunctions of the catalyst must occur within a predefined time interval ⁇ t F.
- the permissible number n F of operating points with a malfunction of the catalytic converter, the number of selected operating points n A and their position, the time interval ⁇ t F and the size of the parameters .DELTA.T G and r CO, G also depend on the type of engine and catalyst the OBD legislation regulations. According to the invention, it is not possible to fix the parameters ⁇ T G and r CO, G as constant values, but to store them as a characteristic field as a function of load and rotational speed in the OBD electronics.
- the typical, measured carbon monoxide emissions of a vehicle during a defined driving cycle (MVEG-A / 2) as a function of the measured CO light-off temperature T CO, 50% of a diesel oxidation catalyst at different aging stages in continuous operation are indicated.
- Emission legislation requires maximum emissions within one driving cycle.
- the maximum allowable emission of CO in the MVEG-A / 2 cycle from 2005 (EU IV standard) is 0.5 g / km.
- the EU IV limit values are no longer met for the example shown in FIG.
- the limit value .DELTA.T G of the temperature difference .DELTA.T can now be selected so that the catalyst according to the above conditions is considered severely damaged if the legal emission limit values are exceeded.
- OBD limit values to be defined by the legislator may also be used.
- the curve shown as an example in FIG. 3 varies depending on the catalyst design, drivability, vehicle type and engine type.
- the OBD method presented here can be adapted to all vehicle types, engine types and legislation.
- FIG. 4 shows the diagram corresponding to FIG. 3 for the behavior of the hydrocarbon emissions recorded on the same vehicle under identical measuring conditions with the same aging procedure. Since no fixed limit value for HC emissions is specified in the European legislation, but instead two limit values for the sum of the NO x and HC emissions and for the NO x emissions, is shown in FIG. 4 as the limit line for the HC Emissions the difference of these two limits drawn.
- FIG. 4 shows that the HC light-off temperature T HC, 50% of the catalyst does not rise to the same extent as the CO light-off temperature T CO, 50% when aged in continuous operation.
- the increase in HC light-off temperature T HC, 50% is not associated with an increase in emissions as much as carbon monoxide; For example, even the difference between the two limit values for HC + NOx and NOx is not exceeded even after a vehicle has been operating for more than 40,000 km. Therefore, according to the invention, CO is selected as the indicator pollutant for catalyst testing.
- the driver may be given a signal as an error message for the damaged catalytic converter.
- the fault diagnosis that is, the time of the error occurrence and the associated engine operating points can be stored in the OBD electronics.
- the single simultaneous fulfillment of conditions 1 and 2 over a greater time interval than ⁇ t F or at a lower number of operating points than n F , ie in the absence of serious damage, can also be stored in the OBD electronics for later workshop diagnostics without the driver an error signal is transmitted.
- Figure 5 It shows a block diagram for the implementation of the proposed method.
- Reference numeral (1) denotes the Diesel engine in which the fuel is introduced through an injector system (2).
- the Injected amount of fuel is measured by suitable sensors (3) and to the Motor electronics (4), which have a data port (I / O), a processor (CPU) and a Memory (RAM) has been transmitted.
- the engine electronics also receives by a suitable sensor system (5) constantly information about the current engine speed, so from the fuel injection quantity and the speed by comparison with an in the engine electronics stored map the load can be calculated.
- This Load and speed operating point information is sent to the OBD electronics (6), which also has data port (I / O), processor (CPU) and memory (RAM).
- the exhaust gas of the engine is via the exhaust pipe (7) to the exhaust gas purification converter (8), in which a suitable catalyst is arranged, directed.
- the reference numerals (9) and (10) designate the sensors for carbon monoxide, its concentration in front of and behind the catalyst to determine the degree of conversion is measured, the sensor (9) depending on the embodiment of the Method is optional.
- (11) denotes a temperature sensor in the immediate spatial proximity to the sensor (10) is arranged in the exhaust line.
- the signals of the CO sensors (9) and (10) and the temperature sensor (11) are sent to the OBD electronics (6) forwarded.
- the OBD electronics receives more sensors and Signal lines (12) Information about all other exhaust gas relevant components of the Engine, the fuel system and the exhaust system.
- FIG. 6 explains by way of example with reference to a flowchart such as a serious one Damage to the catalyst determined according to the inventive method can be. Within the scope of the claims are other variants of this procedure possible.
- Reference number (100) designates the start of the procedure, which is monitored and controlled by a sequence program stored in the OBD electronics.
- step (102) first the time measurement t and the number n of the stored operating points with a malfunction of the catalytic converter are set to zero.
- step (103) the time measurement is started, whereupon in step (104) the current engine operating point (BP) is recorded from load and speed. It is checked in step (105) whether the current operating point is an element of the set BP A (BP ⁇ BP A ?) Of the operating points selected for the evaluation of the catalytic converter and stored in the OBD electronics. If this is not the case, the recording of a new operating point is continued (104).
- step (106) it is checked in step (106) whether the current operating point BP already belongs to the set of previously stored operating points BPF for which a malfunction of the catalytic converter has been detected or differs therefrom. If a malfunction has already been detected for this operating point, step (104) is continued. Otherwise, the measurement of the current exhaust gas temperature T A is made behind the catalytic converter in step (107). In step (108), it is then checked whether the current exhaust gas temperature T A is greater than the sum of the CO light-off temperature T CO, 50% fresh of the fresh catalyst and the limit value of the temperature difference .DELTA.T G. If this is not the case, the recording of a new operating point is continued in step (104). Otherwise, the measurement of the carbon monoxide concentration is made in step (109).
- step (102) is continued, that is, the time count and the stored operating points with malfunction are reset. If, on the other hand, the time interval has not yet been exceeded, it is checked in step (113) whether the permissible number n F of operating points with malfunction has already been reached. If this is not already the case, the recording of further operating points is continued in step (104). If the permissible number of operating points is exceeded, this is stored in step (114) in the OBD electronics as serious damage to the catalytic converter and an error signal is output in step (115).
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Combustion & Propulsion (AREA)
- Mechanical Engineering (AREA)
- General Engineering & Computer Science (AREA)
- Exhaust Gas After Treatment (AREA)
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
- Combined Controls Of Internal Combustion Engines (AREA)
- Catalysts (AREA)
- Investigating Or Analyzing Non-Biological Materials By The Use Of Chemical Means (AREA)
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE10013893A DE10013893A1 (de) | 2000-03-21 | 2000-03-21 | Verfahren zur Überprüfung der Funktionstüchtigkeit eines Abgasreinigungskatalysators |
DE10013893 | 2000-03-21 |
Publications (2)
Publication Number | Publication Date |
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EP1136671A1 EP1136671A1 (de) | 2001-09-26 |
EP1136671B1 true EP1136671B1 (de) | 2003-07-09 |
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Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
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EP01106782A Expired - Lifetime EP1136671B1 (de) | 2000-03-21 | 2001-03-17 | Verfahren zur Überprüfung der Funktionstüchtigkeit eines Abgasreinigungskatalysators |
Country Status (16)
Country | Link |
---|---|
US (1) | US6739176B2 (ru) |
EP (1) | EP1136671B1 (ru) |
JP (1) | JP4625194B2 (ru) |
KR (1) | KR100592695B1 (ru) |
CN (1) | CN1231659C (ru) |
AR (1) | AR027648A1 (ru) |
AT (1) | ATE244816T1 (ru) |
AU (1) | AU2809401A (ru) |
BR (1) | BR0101110B1 (ru) |
CA (1) | CA2341065C (ru) |
CZ (1) | CZ2001882A3 (ru) |
DE (2) | DE10013893A1 (ru) |
ES (1) | ES2197130T3 (ru) |
PL (1) | PL346557A1 (ru) |
RU (1) | RU2267619C2 (ru) |
ZA (1) | ZA200102335B (ru) |
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DE102008008985A1 (de) * | 2008-02-13 | 2009-08-20 | Volkswagen Ag | Verfahren zur OSC-basierten Diagnose eines Katalysators |
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DE4211092A1 (de) * | 1992-04-03 | 1993-10-07 | Bosch Gmbh Robert | Verfahren und Vorrichtung zum Beurteilen der Funktionsfähigkeit eines Katalysators |
JP3157061B2 (ja) * | 1993-04-26 | 2001-04-16 | 株式会社日立製作所 | 触媒劣化診断システム |
JP3082523B2 (ja) * | 1993-08-09 | 2000-08-28 | 日産自動車株式会社 | 内燃機関の触媒劣化診断装置 |
JP3830568B2 (ja) * | 1995-12-18 | 2006-10-04 | 日本碍子株式会社 | 排気ガス浄化触媒の劣化検知方法 |
US5732551A (en) | 1996-12-11 | 1998-03-31 | Motorola Inc. | Method for monitoring the performance of a catalytic converter using mass transfer coefficients |
US5941918A (en) | 1997-07-30 | 1999-08-24 | Engelhard Corporation | Automotive on-board monitoring system for catalytic converter evaluation |
US6026639A (en) * | 1997-11-03 | 2000-02-22 | Engelhard Corporation | Apparatus and method for diagnosis of catalyst performance |
JP2001317345A (ja) * | 2001-04-02 | 2001-11-16 | Hitachi Ltd | エンジンの排気浄化装置 |
-
2000
- 2000-03-21 DE DE10013893A patent/DE10013893A1/de not_active Withdrawn
-
2001
- 2001-03-09 CZ CZ2001882A patent/CZ2001882A3/cs unknown
- 2001-03-13 AR ARP010101162A patent/AR027648A1/es unknown
- 2001-03-16 US US09/809,355 patent/US6739176B2/en not_active Expired - Lifetime
- 2001-03-17 AT AT01106782T patent/ATE244816T1/de not_active IP Right Cessation
- 2001-03-17 ES ES01106782T patent/ES2197130T3/es not_active Expired - Lifetime
- 2001-03-17 DE DE50100354T patent/DE50100354D1/de not_active Expired - Lifetime
- 2001-03-17 EP EP01106782A patent/EP1136671B1/de not_active Expired - Lifetime
- 2001-03-19 CA CA002341065A patent/CA2341065C/en not_active Expired - Fee Related
- 2001-03-19 AU AU28094/01A patent/AU2809401A/en not_active Abandoned
- 2001-03-20 KR KR1020010014345A patent/KR100592695B1/ko not_active IP Right Cessation
- 2001-03-20 PL PL01346557A patent/PL346557A1/xx unknown
- 2001-03-20 RU RU2001107267/06A patent/RU2267619C2/ru not_active IP Right Cessation
- 2001-03-20 ZA ZA200102335A patent/ZA200102335B/xx unknown
- 2001-03-21 CN CNB011097183A patent/CN1231659C/zh not_active Expired - Fee Related
- 2001-03-21 JP JP2001081491A patent/JP4625194B2/ja not_active Expired - Fee Related
- 2001-03-21 BR BRPI0101110-3A patent/BR0101110B1/pt not_active IP Right Cessation
Cited By (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE102004004277A1 (de) * | 2004-01-27 | 2005-09-22 | Audi Ag | Verfahren zur Beurteilung der Güte eines einer Brennkraftmaschine eines Fahrzeuges, insbesondere eines Kraftfahrzeuges, nachgeschalteten Abgaskatalysators |
DE102008008985A1 (de) * | 2008-02-13 | 2009-08-20 | Volkswagen Ag | Verfahren zur OSC-basierten Diagnose eines Katalysators |
DE102008008985B4 (de) * | 2008-02-13 | 2017-08-31 | Volkswagen Ag | Verfahren zur OSC-basierten Diagnose eines Katalysators |
DE102009021991A1 (de) | 2009-05-19 | 2010-11-25 | Volkswagen Ag | Verfahren zur Bestimmung einer Anspringtemperatur und/oder eines Anspringverhaltens eines Katalysators |
RU2564687C2 (ru) * | 2011-07-11 | 2015-10-10 | Сканиа Св Аб | Способ и устройство для тестирования жидкости |
Also Published As
Publication number | Publication date |
---|---|
RU2267619C2 (ru) | 2006-01-10 |
JP4625194B2 (ja) | 2011-02-02 |
US20010033815A1 (en) | 2001-10-25 |
AR027648A1 (es) | 2003-04-09 |
JP2001336415A (ja) | 2001-12-07 |
KR20010092397A (ko) | 2001-10-24 |
CA2341065A1 (en) | 2001-09-21 |
KR100592695B1 (ko) | 2006-06-23 |
US6739176B2 (en) | 2004-05-25 |
ES2197130T3 (es) | 2004-01-01 |
ZA200102335B (en) | 2001-09-21 |
CN1231659C (zh) | 2005-12-14 |
CZ2001882A3 (cs) | 2001-11-14 |
BR0101110B1 (pt) | 2011-12-13 |
CN1314544A (zh) | 2001-09-26 |
PL346557A1 (en) | 2001-09-24 |
CA2341065C (en) | 2008-05-20 |
EP1136671A1 (de) | 2001-09-26 |
DE50100354D1 (de) | 2003-08-14 |
ATE244816T1 (de) | 2003-07-15 |
DE10013893A1 (de) | 2001-09-27 |
BR0101110A (pt) | 2001-11-06 |
AU2809401A (en) | 2001-09-27 |
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